Available online at www.sciencedirect.
com Current Opinion in
ScienceDirect
Nanomaterials and catalysis for green chemistry
Paulette Gómez-López1, Alain Puente-Santiago2,
Andrés Castro-Beltrán3, Luis Adriano Santos do Nascimento4,
Alina M. Balu1, Rafael Luque1,5 and
Clemente G. Alvarado-Beltrán3
Recently, green chemistry for the development of sustainable
production systems requires tremendous research efforts on
the design of catalysts through resource-efficient ways. The
improvement of their catalytic performances is a key goal in
modern society. Several approaches using environmentally
friendly chemicals and materials for less hazardous synthesis
and catalysis were analyzed. In this review, we focus on the
synthesis of nanomaterials and catalytic applications to reduce
the environmental impact, especially, by reducing waste, sol-
vents, precursors, and derivatives. In addition, we highlight the
special efforts toward the use of renewable feedstocks and
their applications as well as the synthetic routes to develop
nanocatalysts using a greener chemistry.
Addresses
1
Departamento de Química Orgánica, Universidad de Cordoba,
Campus de Rabanales, Edificio Marie Curie (C-3), Ctra Nnal IV-A, Km
396, E14014, Cordoba, Spain
2
Department of Chemistry and Biochemistry, University of Texas at El
Paso, 500 W. University Avenue, El Paso, TX 79968, USA
3
Facultad de Ingeniería Mochis, Universidad Autónoma de Sinaloa,
Fuente de Poseidón y Prol. Angel Flores, S.N., 81223, Los Mochis Sin,
Mexico
4
Laboratory of Amazon Oils and Graduate Program of Chemistry,
Federal University of Pará, Rua Augusto Corrêa, Guamá, CEP, 66075-
110, Belém, Pará, Brazil
5
Scientific Center for Molecular Design and Synthesis of Innovative
Compounds for the Medical Industry, People's Friendship University of
Russia (RUDN University), Moscow, Russia
Corresponding authors: Alvarado Beltrán, Clemente G (calvarado@
uas.edu.mx); Luque, Rafael, (q62alsor@uco.es)
Current Opinion in Green and Sustainable Chemistry 2020,
24:48–55
This review comes from a themed issue on Green and Sustainable
nanotechnology
Edited by Alina Balu and Daily Rodríguez-Padrón
https://doi.org/10.1016/j.cogsc.2020.03.001
2452-2236/© 2020 Elsevier B.V. All rights reserved.
Introduction
Nowadays, the research endeavors have been focused on
reconfiguring the process to provide materials and
energy, avoiding the generation of high volume of waste,
hazard derivatives, and source consumption. With regard
Current Opinion in Green and Sustainable Chemistry 2020, 24:48–55
Green and Sustainable Chemistry
to this, the design, development, and synthesis of new
catalysts are the key to improving the performance of
fine chemistry [1]. Several approaches have been widely
explored to obtain the ideal catalyst with stability,
selectivity, and high activity properties at the same time,
which is still being a challenge [2]. Among the various
strategies, the recent studies focusing on developing
nanomaterials by green procedures are acquiring pivotal
position. In this review, the synthesis of new nano-
materials by the solvent-free process, green synthesis,
and, also, the use of natural extracts and organic sup-
ports has been widely discussed. In addition, the cata-
lytic application of the most relevant nanomaterials in
renewable feedstock production for sustainable process
was analyzed.
Solvent-free synthesis of porous
nanomaterials
The porous materials are very attractive because of their
properties such as high surface area, tunable acidity,
ordered micropores, active site access, and stability. For
example, SBA-15, MCM-41, zeolites, and metal-organic
framework (MOF) structures are highly used in catalytic
process because they can be used as support. The syn-
thesis of supported nanoparticles (NPs) allows good
dispersion, controls allocation of active sites, and con-
tributes to NP stabilization. The mechanochemical
method have emerged as a green method because they
allow solvent-free synthesis of the catalyst supported on
mesoporous material, especially metal oxide NPs,
compared with wet impregnation or coprecipitation. As
proof of that, Saberia et al [3] synthetized Fe2O3/SBA-
15, for which Fe(NO3)3$H2O and propionic acid were
dispersed using a planetary ball mill and then calcined at
300
C for 30 min (Figure 1a). The nanomaterial was
magnetically separable with a high surface area
(SBET = 322 m2/g) [3]. But previously,
nonmagnetic FeeSBA-15 modified by sulfonic groups
was reported [4]. Moreover, to enhance the catalytic
properties, Pineda et al. [5] supported Co3O4 on SBA-
15, achieving a bifunctional nanomaterial with redox and
acid sites, with an SBET of 625 m2/g. Following the same
route, Au and Ag were also supported on SBA-15 [6].
Similarly, Al species were supported on SBA-15, MCM-
41, and MOF. The green synthesis route presented less
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Figure 1
Free-solvent routes for mesoporous nanomaterials. Based on the studies by (a) [3] for SBA-15 and MCM-41, (b) [7] for zeolites, and (c) [10] mesoporous
nanomaterial.
acidity and lower superficial area than the impregnation
method [6].
Outstandingly, zeolite synthesis has been achieved
through the solvent-free method. For instance, Zhang et
al [7] reported the synthesis of ZSM-5 from rice husk
ash, TPABr/SiO2, and Na2CO3$10H2O/SiO2 mixture,
pretreated them into an autoclave at 150
C for 72 h,
and later calcined at 550
C for 6 h to remove the organic
template (Figure 1b). They present similar character-
istic when it is synthetized by solvent-free method SBET
= 304 m2/g or hydrothermal process SBET = 320 m2/g
[7]. In addition, hierarchical zeolite Co particles
entrapped inside ZSM-5 with great crystallinity and
high surface area higher than a SBET of 200 m2/g were
reported [8].
Massive efforts have been devoted toward synthesis of
encapsulated NP materials by solvent-free methods.
The mechanochemical method allows the NPs in the
MOF matrices through solid-state reaction during the
sacrificial process. As a result, Pd NPs in ZIF-8 crystal by
ball milling, without stabilizing agents was done [9].
The nanomaterials present a good crystalline structure
with a high surface area of more than 1300 m2/g. In
addition, a mesoporous Pteiron oxide mechanochemical
assembly was synthetized by a simple and rapid solvent-
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Catalysis for green chemistry Gómez-López et al. 49
free method (Figure 1c). The iron salt and triblock
copolymer in the solid-state reaction for 0.5 h allows a
narrow pore size distribution and high surface area
(149 m2/g) with well-dispersed Pt [10].
Green synthesis of two-dimensional
materials
The two-dimensional (2D) materials have been
continuously revolutionizing the materials science field
in the last years [11]. They are formed by a sheet-like
structure composed from a single atomic layer to a few
number of layers, which can be used to tune their
physical, chemical, optical, and electronic properties
[12]. In addition, they have become essential materials
toward the fabrication of a myriad of high-performance
devices from ultraefficient electrocatalysts [13] and
flexible/wearable (opto)electronics to energy harvesting
and sensing technologies owing to their unique physical
and chemical properties [14,15]. Nevertheless, exten-
sive research has not been conducted on the develop-
ment of sustainable and eco-friendly synthetic
approaches to create 2D materials.
In this direction, with the aim to obtain highly sus-
tainable 2D nanostructured materials, various research
groups have recently delivered significant endeavors.
Remarkably, Pei et al. [16] have reported a green,
Current Opinion in Green and Sustainable Chemistry 2020, 24:48–55
50 Green and Sustainable nanotechnology
Figure 2
Schematic illustration of eco-friendly synthetic methodologies toward the synthesis of innovative 2D materials, Adapted from (a) [16], (b) [17], (c) [18],
(d) [19].
innovative, and ultrafast methodology to fabricate high-
quality graphene oxide (GO) sheets by water electro-
lytic oxidation of graphite. The synthesis was carried out
at room temperature following two electrochemical
(EC) steps (Figure 2). First, a high potential of 1.6 V for
20 min was applied over commercial flexible graphite
samples immersed in H2SO4 (98%) solutions to trigger
an EC intercalation process (Figure 2a). Second, the
resulting compound was used as the anode in diluted
H2SO4 (50%) solutions to start an EC reaction at 5 V, at
which the oxygen radicals of the anodic electrocatalytic
oxygen evolution reaction play a key role in the forma-
tion of GO layers with low oxidation degree. Another
attractive strategy to synthesize low-dimensional nano-
materials using environmentally friendly process is
based on the sonication of Ni2þ and Fe2þ in the pres-
ence of MoS2 as 2D templates [17]. Following this
methodology, 2D/2D heterostructures composed of
NiFe nanosheets onto MoS2 layers are fabricated taking
advantage of the weak van der Waals interactions at the
2D interfaces (Figure 2b). In addition, an impressive
approach to obtain high yields of 2D MOFs was pro-
posed by Zhang. et al [18]. They established a
surfactant-mediated methodology in which the inter-
action of the surfactant with MOF crystal defects
Current Opinion in Green and Sustainable Chemistry 2020, 24:48–55
provides a pseudoassembly process to exfoliate the 3D
MOFs and in turn produce 2D sheets (Figure 2c) [18].
Substantial advances have been also achieved on the
green fabrication of MXenes nanosheets, a relatively
new promising 2D material. In this direction, Zhang et
al [19] have developed a simple template-free method
by liquid rapid freezing in nitrogen (Figure 2d), paving
the way toward the fabrication of low-cost 3D micro-
porous structured MXenes.
Green synthesis of metal and metal
oxide NPs using plant extracts
In the last years, the use of NPs essentially in the
catalysis industry is still increasing. The development of
metal-based NPs has been widely explored for many
physical and chemical methods [20]. Recently, there has
been an increase in the number of research studies using
environmental friendly approaches. Particularly, green
synthesis has become a successfully alternative to
traditional process because of the reduction in the use of
reducing agents, surfactants, and stabilizers without
generation of toxic derivative compounds [21].
Regarding this, the use of natural extract from plants to
synthetize inorganic NPs is a simple, economic-effi-
cient, and sustainable route. Principally, the extracts
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Figure 3
The green synthesis route to obtain nanoparticles using plants extracts.
from leaves, seeds, roots, flowers, and fruits have been
used (Figure 3). The extracts are composed of phyto-
chemicals such as protein, amino acids, vitamins, poly-
saccharides, terpenoids, and organic acids [22],
which act as a natural reducing agent and stabilizer in
situ, important for shape and size control. As a result,
noble metals such as gold and silver NPs are the most
common used in catalytic industry because of their high
catalytic reduction, antibacterial, and optoelectronic
properties. For instance, Girón-Vázquez et al [23]
synthetized Ag NPs by varying extract concentration of
Persea americana seeds, and they found a
correlation between higher concentration of extracts
and higher size. Remarkably, Anandan et al [24] re-
ported the size and shape control of Ag NPs. For that,
different solvents were used to obtain Dodonaea viscosa
leaf extracts. Furthermore, Au NPs were synthesized
using leaf extracts of Annona muricata [25]. In this route,
Bogireddy et al [26] studied the pH effect of the Coffea
arabica seed extract on size control. And the results are
similar to those obtained when NaBH4 is used as a
reducing agent. In addition, Au NP size increases with
reaction time, using Agave potatorum extract [27].
Similarly, green synthesis of metal oxide NPs has also
been achieved. As an example, the extract concentration
of Lycopersicon esculentum peel affects the size and the
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Catalysis for green chemistry Gómez-López et al. 51
homogeneity of ZnO and SnO2 NPs [28e30]. In addi-
tion, the concentration of Daucus carota extract modified
the ZnO band gap, crystallinity, and crystal size [31].
Likewise, Calotropis gigantea leaf extract acts as a
reducing agent and stabilizer in SnO2 synthesis [32].
Leaf extracts of Jatropha curcas [33] and Lippia [34],
were used in the synthesis of TiO2. The last
one resulted in TiO2 in two phases: 85% anatase and
15% rutile, with a size of 20e40 nm. On the other hand,
pure TiO2 was achieved using cinnamon powder extract,
with spherical shape and a size between 50 and 100 nm
[35].
Green synthesis of organic-based materials
Nanocomposites based on organic materials have been
extensively studied in recent years [36]. They have
been synthetized using a myriad of bioinspired materials
as renewable alternatives to reduce the use of hazard
chemicals and derivatives. The synthesized materials
showed high surface areas, which is very attractive for
catalytic applications owing to their unique highly
porous structures with active sites, particularly those
decorated by metal and metal oxide NPs. In this di-
rection, new approaches are described in the literature
including copolymerization of two types of monomers
under solvothermal reaction conditions (generating a
Current Opinion in Green and Sustainable Chemistry 2020, 24:48–55
52 Green and Sustainable nanotechnology
new N-rich porous organic polymer), followed by a
subsequent incorporation of palladium NPs [37].
Natural materials such as starch, chitosan (CH)/chitin,
lignin, and cellulose have been reported as renewable-
derived polymers for the preparation of active nano-
catalysts (Figure 4). For example, Sadjadi et al [38]
synthesized a biocompatible nanomaterial based on the
immobilization of palladium (II) acetate on a starche
halloysite hybrid system. Starch was also successfully
used to create a green composite with CH, which
stabilized palladium NPs [39]. CH has also been used
as a biopolymer in the production of biocide formula-
tions composed of ZnO-interlinked CH NPs [40]. In
another report, new biomass-derived catalysts from
lignin pyrolysis with metals could provide access to Co/
Mnelignin complexes and dicyandiamide that encap-
sulates cobalt NPs [41]. Furthermore, lignin and chitin
have been used to synthesize magnetic biocatalytic
systems composed of trypsin immobilized on magne-
tite NPs [42]. In addition, cellulose nanocrystals were
used as supports for nucleation of silver and gold NPs
via solid-state synthesis using a solvent-free method
[43].
Figure 4
Organic materials, polymer-derived paths, and their modifications. NP, nanoparticle.
Current Opinion in Green and Sustainable Chemistry 2020, 24:48–55
As a very innovative strategy, the transformation of waste
fractions from saw mills to supporting preformed metal
AuePt NPs rendered catalytically active materials [44].
In the same route, Lisowski et al [45] presented, for the
first time, the use of low-temperature ultrasonic-assis-
ted solegel method coupled to produce crystalline TiO2
NPs from lignocellulosic biomass. In addition, inter-
connected carbon sheet networks with hierarchical
porous structures were generated from steam-exploded
wheat straw, while FeCl3$6H2O gives rise to magnetic
NPs uniformly embedded in porous carbon foams [46].
Coffee ground spent has been used to obtain magnetic
nanocatalysts by ammonium iron (III) citrate incorpo-
ration through mechanochemical milling followed by
calcination [47]. In the same route, proteinetemplate
TiO2 used expired eggs as the biomass-derived source
[48]. In addition, a magnetically separable biosystem
based on laccase-functionalized waste-derived Fe2O3
was successfully achieved [49].
Catalysis for renewable feedstocks
Undoubtedly, the enthusiasm to improve strategies for
the use of renewable feedstocks as an alternative to
traditional industry resource needs to be materialized.
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The traditional industry based on oil-derived platform
chemicals, such as ethene, propene, benzene, and xy-
lenes, is in depletion. As a result, new platform chemicals
derived from biomass such as 5-hydroxymethylfurfural
(HMF), levulinic acid (LA), furfurals, glycerol, sugar
alcohols, lactic acid, succinic acid, and phenols have been
proposed as renewable feedstocks. The building block
chemicals are used to create a new compound by
upgrading reactions. Processes such as hydrogenation,
oxidation, alkylation, esterification, and others are used
to produce value-added chemicals. As representative
biomass-based platform molecules, HMF has been
commonly used to produce 2,5-furandicarboxylic acid
(FDCA) among other intermediate chemicals. FDCA is
a value-added chemical substitute to produce polyesters,
polyamides, polyurethanes, and, principally, poly-
ethylene furanoate and is the best alternative to
petroleum-derived polyethylene terephthalate. Fang et
al [50] reported the catalytic activity of ultrafine cobalt
oxide NPs encapsulated within mesopores of KIT-6 in
biomass-derived HMF oxidation under mild reactions
conditions, achieving a complete conversion and >99%
FDCA selectivity even after 6 runs. In addition, Zhou et
al [41] reported CoeMnelignin coordination
complex materials for HMF oxidation using O2 in H2O as
a green oxidant source with 99.5% HMF conversion and
92.7% FDCA selectivity even after 6 runs.
Actually, as sugar-derived building blocks, LA is
considered one of the most promising platform mole-
cules. LA valorization is carried out to produce more
valuable products, that is, by hydrogenation to convert
into g-valerolactone and N-heterocycles. For instance,
Zhang et al [51] reported the hydrogenation of LA using
the CuAg/Al2O3 bimetallic catalyst, achieving almost
100% yield to g-valerolactone even after nine consecu-
tive runs. In addition, Rodriguez-Padrón et al [52] pro-
posed LA as the building block to
synthetize polyrridones, especially, 1-ethyl-5-
methylpyrrolidin-2-one. Reductive amination of LA
driven by g-C3N4/Pt composites, under flow chemistry,
with an effective reaction mixing LA and 1,4-dicarbonyl
compounds reported a selectivity higher than 60% [52].
Conclusions and perspectives
A number of research efforts have been taken to obtain
sustainable nanomaterials by exploring different green
synthetic routes. Currently, the performance of syn-
thesized nanomaterials is far from ideal, whereas the
green synthesis and sustainable processes for catalyst
and chemical production are closer. The drawbacks of
the catalyst such as recovery issue are usually present,
with fewer number of runs, poisoning, and leaching
being the most frequently reported. There are great
endeavors to prepare nanomaterials by means of green
paths using more abundant metals such as Co and Cu,
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Catalysis for green chemistry Gómez-López et al. 53
supported on natural polymer with N-rich sites with
remarkable performances. In addition, the performance
of nanomaterials modified with Fe2O3 and Co3O4
phases is extremely relevant because they can be
magnetically separated for easy and efficient recovery.
Undoubtedly, the natural source and biomass-based
compounds are the key to developing more sustain-
able and efficient nanocatalysts. In summary, to achieve
that goal, serious efforts must be addressed to obtain
catalysts with excellent properties such as high stabil-
ity, selectivity, and activity using green synthetic
approaches.
Conflict of interest statement
Nothing declared.
Acknowledgements
CGA-B gratefully acknowledges support from PRODEP (SEP-UAS) for the
professor visiting program. PG-L gratefully acknowledges support of
CONACYT-México for the international fellowship number 709621. RL
acknowledges funding from MINECO under project CTQ2016-78289-P.
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28. Sotoo-Robles CA, Nava OJ, Vilchiso-Nestor AR, Castroo-
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29. Garrafa-Galvez HE, Nava O, Soto-Robles CA, Vilchis-Nestor AR,
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35. Nabi G, Raza W, Tahir MB: Green synthesis of TiO2 nano-
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for the efficient inhibition of sulfate-reducing bacteria in
inject seawater. ACS Sustainable Chem Eng 2018, 6:
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A new biomass-derived catalysts Co/Mn-lignin was synthetized. The
catalyst was tested in for HMF oxidation with conversion of 99.5% and
FDCA selectivity of 92.7% even after 6 runs. A very active catalyst for
biomass derived molecules plattforms were reported.
42. Zdarta J, Antecka K, Jedrzak A, Synoradzki K, Łuczak M,
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47. Rodríguez-Padrón D, Batista MJ, Li H, Shih K, Balu AM,
Pineda A, Luque R: Spent coffee grounds-templated magnetic
nanocatalysts for mild oxidations. ACS Sustainable Chem Eng
2019, 7:17030–17038. https://doi.org/10.1021/
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48. Rodríguez-Padrón D, Puente-Santiago AR, Luna-Lama F,
Caballero A, Batista MJ, Luque R: Versatile protein-templated
TiO2 nanocomposite for energy storage and catalytic appli-
cations. ACS Sustainable Chem Eng 2019, 7:5329–5337.
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49. Rodríguez-Padrón D, Puente-Santiago AR, Caballero A,
* Balu AM, Romero AA, Luque R: Highly efficient direct oxygen
electro-reduction by partially unfolded laccases immobilized
on waste-derived magnetically separable nanoparticles.
Nanoscale 2018, 10:3961–3968. https://doi.org/10.1039/
C8NR00512E.
The authors demonstrated the synthesis a magnetically separable
biosystem. The green route includes the laccase functionalization with
Fe2O3. The nanomaterial is catalytic active, also is magnetically
attractive for products separation and recovery.
50. Fang R, Tian P, Yang X, Luque R, Li Y: Encapsulation of ul-
* * trafine metal-oxide nanoparticles within mesopores for
biomass-derived catalytic applications. Chem Sci 2018, 9:
1854–1859. https://doi.org/10.1039/c7sc04724j.
The authors report the catalytic activity of ultrafine Cobalt-oxide NPs
encapsulated within mesopores of KIT-6. The activity tested in
biomass-derived HMF oxidation under mild reactions conditions,
achieving a complete conversion and >99% FDCA selectivity even
after 6 runs. The material is very attractive for catalytic applications.
51. Zhang L, Mao J, Li S, Yin J, Sun X, Guo X, Song C, Zhou J:
Hydrogenation of levulinic acid into gamma-valerolactone
over in situ reduced CuAg bimetallic catalyst: strategy and
mechanism of preventing Cu leaching. Appl Catal B: Environ
2018, 232:1–10. https://doi.org/10.1016/j.apcatb.2018.03.033.
52. Rodríguez-Padrón D, Puente-Santiago AR, Balu AM, Muneoz-
Batista MJ, Luque Rafael: Continuous flow synthesis of high
valuable N-heterocycles via catalytic conversion of levulinic
acid. Front Chem 2019, 7:103. https://doi.org/10.3389/
fchem.2019.00103.
Current Opinion in Green and Sustainable Chemistry 2020, 24:48–55